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期刊信息/Journal information
能源化学
能源化学

包信和 ALEXIS T.BELL

双月刊

2095-4956

jngc@dicp.ac.cn

0411-84379237

116023

大连市中山路457号

能源化学/Journal Journal of Energy ChemistryCSCDCSTPCD北大核心EISCI
查看更多>>本刊旨在报道世界范围内天然气化学及其相关领域的最新发展动态和科技信息，增进国际交流，促进科技发展。以天然气及其相关领域从事化学和化学工程方面研究的科研人员及工程技术人员、大专院校的本科生、研究生和教师等为读者对象。
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    Rationally designing electrolyte additives for highly improving cyclability of LiNi0.5Mn1.5O4/Graphite cells

    Zhiyong XiaKuan ZhouXiaoyan LinZhangyating Xie...
    266-275页
    查看更多>>摘要：High voltage is necessary for high energy lithium-ion batteries but difficult to achieve because of the highly deteriorated cyclability of the batteries.A novel strategy is developed to extend cyclability of a high voltage lithium-ion battery,LiNi0.5Mn1.5O4/Graphite(LNMO/Graphite)cell,which emphasizes a rational design of an electrolyte additive that can effectively construct protective interphases on anode and cathode and highly eliminate the effect of hydrogen fluoride(HF).5-Trifluoromethylpyridine-trime thyl lithium borate(LTFMP-TMB),is synthesized,featuring with multi-functionalities.Its anion TFMP-TMB-tends to be enriched on cathode and can be preferentially oxidized yielding TMB and radical TFMP.Both TMB and radical TFMP can combine HF and thus eliminate the detrimental effect of HF on cathode,while the TMB dragged on cathode thus takes a preferential oxidation and constructs a protec-tive cathode interphase.On the other hand,LTFMP-TMB is preferentially reduced on anode and con-structs a protective anode interphase.Consequently,a small amount of LTFMP-TMB(0.2％)in 1.0 M LiPF6 in EC/DEC/EMC(3/2/5,wt％)results in a highly improved cyclability of LNMO/Graphite cell,with the capacity retention enhanced from 52％to 80％after 150 cycles at 0.5 C between 3.5 and 4.8 V.The as-developed strategy provides a model of designing electrolyte additives for improving cyclability of high voltage batteries.
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    Morphology and valence state evolution of Cu:Unraveling the impact on nitric oxide electroreduction

    Ting SunFengyu GaoYa WangHonghong Yi...
    276-286页
    查看更多>>摘要：Ammonia(NH3)serves as a critical component in the fertilizer industry and fume gas denitrification.However,the conventional NH3 production process,namely the Haber-Bosch process,leads to consider-able energy consumption and waste gas emissions.To address this,electrocatalytic nitric oxide reductionreaction(NORR)has emerged as a promising strategy to bridge NH3 consumption to NH3 production,har-nessing renewable electricity for a sustainable future.Copper(Cu)stands out as a prominent electrocat-alyst for NO reduction,given its exceptional NH3 yield and selectivity.However,a crucial aspect that remains insufficiently explored is the effects of morphology and valence states of Cu on the NORR perfor-mance.In this investigation,we synthesized CuO nanowires(CuO-NF)and Cu nanocubes(Cu-NF)as cath-odes through an in situ growth method.Remarkably,CuO-NF exhibited an impressive NH3 yield of 0.50+0.02 mg cm-2 h-1 at-0.6 V vs.reversible hydrogen electrode(RHE)with faradaic efficiency of 29.68％+1.35％,surpassing that of Cu-NF(0.17+0.01 mg cm-2 h-1,16.18％±1.40％).Throughout the elec-troreduction process,secondary cubes were generated on the CuO-NF surface,preserving their nanosheet cluster morphology,sustained by an abundant supply of subsurface oxygen(s-O)even after an extended duration of 10 h,until s-O depletion ensued.Conversely,Cu-NF exhibited inadequate s-O content,leading to rapid crystal collapse within the same timeframe.The distinctive current-potential relationship,akin to a volcano-type curve,was attributed to distinct NO hydrogenation mechanisms.Further Tafel analysis revealed the exchange current density(i0)and standard heterogeneous rate constant(k0)for CuO-NF,yielding 3.44 × 10-6 A cm-2 and 3.77 × 10-6 cm-2 s-1 when NORR was driven by overpotentials.These findings revealed the potential of CuO-NF for NO reduction and provided insights into the intricate interplay between crystal morphology,valence states,and electrochemical performance.
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    Solar-driven CO2 conversion to methane and methanol using different nanostructured Cu2O-based catalysts modified with Au nanoparticles

    Jo?o Angelo Lima PeriniLilian D.Moura TorquatoJuliana F.de BritoGustavo A.Andolpho...
    287-298页
    查看更多>>摘要：This work describes the use of TiO2 nanotubes-based electrodes(TNT)modified with Cu2O nanostruc-tures and gold nanoparticles for the photoelectroreduction of CO2 to produce value-added compounds.A thin layer of polydopamine was used as both an adherent agent and an electron transfer mediator,due to its π-conjugated electron system.The highest production yield was achieved using a TNT@PDA/Nc/Au40％electrode,with Faradaic efficiencies of 47.4％(110.5 μM cm-2)and 27.8％(50.4 μM cm-2)for methanol and methane,respectively.The performance of the photoelectrodes was shown to be Cu2O facet-dependent,with cubic structures leading to greater conversion of CO2 to methanol(43％)and methane(27％),compared to the octahedral morphology,while a higher percentage of metallic gold on the nanostructured Cu2O surface was mainly important for CH4 production.Density functional theory(DFT)calculations supported these findings,attributing the superior photoelectrocatalytic performance of the TNT@PDA/Nc/Au40％electrode for CH4 generation to the formation of an OCH3 intermediate bonded to Au atoms.Studies using isotope-labeling and analysis by gas chromatograph-mass(GC-MS)demon-strated that 13CO2 was the source for photoelectrocatalytic generation of 13CH3OH and 13CH313CH2OH.
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    High photoelectric conversion efficiency and fast relaxation time of FA0.4MA0.6PbI3 applied in ultrafast modulation of terahertz waves

    Zhibo XuYing ZengXinran ZhaoXiaoyin Chen...
    299-305页
    查看更多>>摘要：Active control of terahertz(THz)waves is attracting tremendous attentions in terahertz communications and active photonic devices.Perovskite,due to its excellent photoelectric conversion performance and simple manufacturing process,has emerged as a promising candidate for optoelectronic applications.However,the exploration of perovskites in optically controlled THz modulators is still limited.In this work,the photoelectric properties and carrier dynamics of FA0.4MA0.6PbI3 perovskite films were investi-gated by optical pumped terahertz probe(OPTP)system.The ultrafast carrier dynamics reveal that FA0.4MA0.6PbI3 thin film exhibits rapid switching and relaxation time within picosecond level,suggesting that FA0.4MA0.6PbI3 is an ideal candidate for active THz devices with ultrafast response.Furthermore,as a proof of concept,a FA0.4MA0.6PbI3-based metadevice with integrating plasma-induced transparency(PIT)effect was fabricated to achieve ultrafast modulation of THz wave.The experimental results demon-strated that the switching time of FA0.4MA0.6PbI3-based THz modulator is near to 3.5 ps,and the thresh-old of optical pump is as low as 12.7 μJ cm-2.The simulation results attribute the mechanism of ultrafast THz modulation to photo-induced free carriers in the FA0.4MA0.6PbI3 layer,which progressively shorten the capacitive gap of PIT resonator.This study not only illuminates the potential of FA0.4MA0.6PbI3 in THz modulation,but also contributes to the field of ultrafast photonic devices.
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    Enhancing the stability of NiFe-layered double hydroxide nanosheet array for alkaline seawater oxidation by Ce doping

    Yongchao YaoShengjun SunHui ZhangZixiao Li...
    306-312页
    查看更多>>摘要：Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy genera-tion.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor ano-dic stability caused by detrimental chlorine chemistry.Herein,we present our recent discovery that the incorporation of Ce into NiFe layered double hydroxide nanosheet array on Ni foam(Ce-NiFe LDH/NF)emerges as a robust electrocatalyst for seawater oxidation.During the seawater oxidation process,CeO2 is generated,effectively repelling Cl-and inhibiting the formation of ClO-,resulting in a notable enhancement in the oxidation activity and stability of alkaline seawater.The prepared Ce-NiFe LDH/NF requires only overpotential of 390 mV to achieve the current density of 1 A cm-2,while maintaining long-term stability for 500 h,outperforming the performance of NiFe LDH/NF(430 mV,150 h)by a sig-nificant margin.This study highlights the effectiveness of a Ce-doping strategy in augmenting the activity and stability of materials based on NiFe LDH in seawater electrolysis for oxygen evolution.
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    High performance wide bandgap perovskite solar cell with low Voc deficit less than 0.4 V

    Haikuo GuoFuhua HouXuli NingXiaoqi Ren...
    313-322页
    查看更多>>摘要：Wide bandgap perovskite solar cells(PSCs)have attracted significant attention because they can be applied to the top cells of tandem solar cells.However,high open-circuit voltage(Voc)deficit(＞0.4 V)result from poor crystallization and high non-radiative recombination losses become a serious limitation in the pursuit of high performance.Here,the relevance between different PbI2 proportions and perfor-mance parameters are revealed through analysis of surface morphology,residual stress,and photostabil-ity.The increase of PbI2 proportion promotes crystal growth and reduces the work function of the perovskite film surface and promotes the energy level alignment with the carrier transport layer,which decreased the Voc deficit.However,residual Pbl2 exacerbated the stress level of perovskite film,and the resulting lattice disorder deteriorated the photostability of the device.Ultimately,after the synergistic passivation of residual PbI2 and PEAI,the Voc achieves 1.266 V and Voc deficit is less than 0.4 V,the record value in wide bandgap PSCs.
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    Internal electric field modulation by copper vacancy concentration of cuprous sulfide nanosheets for enhanced selective CO2 photoreduction

    Xian ShiWeidong DaiXiaoqian LiYang Bai...
    324-330页
    查看更多>>摘要：Although the internal electric field(IEF)of photocatalysts is acknowledged as a potent driving force for photocharge separation,modulating the IEF intensity to achieve enhanced photocatalytic performances remains a challenge.Herein,cuprous sulfide nanosheets with different Cu vacancy concentration were employed to study IEF modulation and corresponding direct charge transfer.Among the samples,Cu1.8S nanosheets possessed intensified IEF intensity compared with those of Cu2S and Cu1.95S nanosheets,suggesting that an enhanced IEF intensity could be achieved by introducing more Cu vacan-cies.This intensified IEF of Cui.8S nanosheets induced numerous photogenerated electrons to migrate to its surface,and the dissociative electrons were then captured by Cu vacancies,resulting in efficient charge separation spatially.In addition,the Cu vacancies on Cu1.8S nanosheets accumulated electrons as active sites to lower the energy barrier of rate-determining step of CO2 photoreduction,leading to the selective conversion of CO2 to CO.Herein,the manipulation of IEF intensity through Cu vacancy con-centration regulation of cuprous sulfide photocatalysts for efficient charge separation has been discussed,providing a scientific strategy to rationally improve photocatalytic performances for solar energy conversion.
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    Ca and Sr co-doping induced oxygen vacancies in 3DOM La2-xSrxCe2-yCayO7-δ catalysts for boosting low-temperature oxidative coupling of methane

    Tongtong WuYuechang WeiJing XiongYitao Yang...
    331-344页
    查看更多>>摘要：It is urgent to develop catalysts with application potential for oxidative coupling of methane(OCM)at relatively lower temperature.Herein,three-dimensional ordered macroporous(3DOM)La2-xSrxCe2-yCayO7-δ(A2B2O7-type)catalysts with disordered defective cubic fluorite phased structure were successfully prepared by a colloidal crystal template method.3DOM structure promotes the acces-sibility of the gaseous reactants(O2 and CH4)to the active sites.The co-doping of Ca and Sr ions in La2-xSrxCe2-yCayO7-δ catalysts improved the formation of oxygen vacancies,thereby leading to increased density of surface-active oxygen species(O2-)for the activation of CH4 and the formation of C2 products(C2H6 and C2H4).3DOM La2-xSrxCe2-yCayO7-δ catalysts exhibit high catalytic activity for OCM at low tem-perature.3DOM La1.7Sr0.3Ce1.7Ca0.3O7-δ catalyst with the highest density of O2-species exhibited the highest catalytic activity for low-temperature OCM,i.e.,its CH4 conversion,selectivity and yield of C2 products at 650 ℃ are 32.2％,66.1％and 21.3％,respectively.The mechanism was proposed that the increase in surface oxygen vacancies induced by the co-doping of Ca and Sr ions boosts the key step of C-H bond breaking and C-C bond coupling in catalyzing low-temperature OCM.It is meaningful for the development of the low-temperature and high-efficient catalysts for OCM reaction in practical application.
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    Polymer engineering for electrodes of aqueous zinc ion batteries

    Zhi PengZemin FengXuelian ZhouSiwen Li...
    345-369页
    查看更多>>摘要：With the increasing demand for scalable and cost-effective electrochemical energy storage,aqueous zinc ion batteries(AZIBs)have a broad application prospect as an inexpensive,efficient,and naturally secure energy storage device.However,the limitations suffered by AZIBs,including volume expansion and active materials dissolution of the cathode,electrochemical corrosion,irreversible side reactions,zinc dendrites of the anode,have seriously decelerated the civilianization process of AZIBs.Currently,poly-mers have tremendous superiority for application in AZIBs attributed to their exceptional chemical sta-bility,tunable structure,high energy density and outstanding mechanical properties.Considering the expanding applications of AZIBs and the superiority of polymers,this comprehensive paper meticulously reviews the benefits of utilizing polymeric applied to cathodes and anodes,respectively.To begin with,with adjustable structure as an entry point,the correlation between polymer structure and the function of energy storage as well as optimization is deeply investigated in respect to the mechanism.Then,depending on the diversity of properties and structures,the development of polymers in AZIBs is summa-rized,including conductive polymers,redox polymers as well as carbon composite polymers for cathode and polyvinylidene fluoride-,carbonyl-,amino-,nitrile-based polymers for anode,and a comprehensive evaluation of the shortcomings of these strategies is provided.Finally,an outlook highlights some of the challenges posed by the application of polymers and offers insights into the potential future direction of polymers in AZIBs.It is designed to provide a thorough reference for researchers and developers working on polymer for AZIBs.
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    Electrochemical reconstruction of non-noble metal-based heterostructure nanorod arrays electrodes for highly stable anion exchange membrane seawater electrolysis

    Jingchen NaHongmei YuSenyuan JiaJun Chi...
    370-382页
    查看更多>>摘要：Direct seawater electrolysis for hydrogen production has been regarded as a viable route to utilize sur-plus renewable energy and address the climate crisis.However,the harsh electrochemical environment of seawater,particularly the presence of aggressive Cl-,has been proven to be prone to parasitic chloride ion oxidation and corrosion reactions,thus restricting seawater electrolyzer lifetime,Herein,hierarchical structure(Ni,Fe)O(OH)@NiCoS nanorod arrays(NAs)catalysts with heterointerfaces and localized oxygen vacancies were synthesized at nickel foam substrates via the combination of hydrothermal and annealing methods to boost seawater dissociation.The hierarchical nanostructure of NiCoS NAs enhanced electrode charge transfer rate and active surface area to accelerate oxygen evolution reaction(OER)and generated sulfate gradient layers to repulsive aggressive Cl-.The fabricated heterostructure and vacancies of(Ni,Fe)O(OH)tuned catalyst electronic structure into an electrophilic state to enhance the binding affinity of hydroxyl intermediates and facilitate the structural transformation into amorphous γ-NiFeOOH for pro-moting OER.Furthermore,through operando electrochemistry techniques,we found that the γ-NiFeOOH possessing an unsaturated coordination environment and lattice-oxygen-participated OER mechanism can minimize electrode Cl-corrosion enabled by stabilizing the adsorption of OH*intermediates,making it one of the best OER catalysts in the seawater medium reported to date.Consequently,these catalysts can deliver current densities of 100 and 500 mA cm-2 for boosting OER at minimal overpotentials of 245 and 316 mV,respectively,and thus prevent chloride ion oxidation simultaneously.Impressively,a highly stable anion exchange membrane(AEM)seawater electrolyzer based on the non-noble metal heterostructure electrodes reached a record low degradation rate under 100 μV h-1 at constant industrial current densities of 400 and 600 mA cm-2 over 300 h,which exhibits a promising future for the non-precious and stable AEMWE in the direct seawater electrolysis industry.
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